First-principles simulations for attosecond photoelectron spectroscopy based on time-dependent density functional theory

We develop a first-principles simulation method for attosecond time-resolved photoelectron spectroscopy. This method enables us to directly simulate the whole experimental processes, including excitation, emission and detection on equal footing. To examine the performance of the method, we use it to compute the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) experiments of gas-phase Argon. The computed RABBITT photoionization delay is in very good agreement with recent experimental results from [Klünder et al., Phys. Rev. Lett. 106, 143002 (2011)] and [Guénot et al., Phys. Rev. A 85, 053424 (2012)]. This indicates the significance of a fully-consistent theoretical treatment of the whole measurement process to properly describe experimental observables in attosecond photoelectron spectroscopy. The present framework opens the path to unravel the microscopic processes underlying RABBITT spectra in more complex materials and nanostructures

Direct Measurement of Electron-Phonon Coupling with Time-Resolved ARPES

Time- and angular- resolved photoelectron spectroscopy is a powerful technique to measure electron dynamics in solids. Recent advances in this technique have facilitated band and energy resolved observations of the effect that excited phonons, have on the electronic structure. Here, we show with the help of ab initio simulations that the Fourier analysis of the time-resolved measurements of solids with excited phonon modes enables the determination of the band- and mode-resolved electron-phonon coupling directly from the experimental data without any additional input from theory. Such an observation is not restricted to regions of strong electron-phonon coupling and does not require strongly excited or hot phonons, but can be employed to monitor the dynamical renormalization of phonons in driven phases of matter

Ab initio simulation of attosecond transient absorption spectroscopy in two-dimensional materials

We extend the first-principles analysis of attosecond transient absorption spectroscopy to two-dimensional materials. As an example of two-dimensional materials, we apply the analysis to monolayer hexagonal boron nitride (h-BN) and compute its transient optical properties under intense few-cycle infrared laser pulses. Nonadiabatic features are observed in the computed transient absorption spectra. To elucidate the microscopic origin of these features, we analyze the electronic structure of h-BN with density functional theory and investigate the dynamics of specific energy bands with a simple two-band model. Finally, we find that laser-induced intraband transitions play a significant role in the transient absorption even for the two-dimensional material and that the nonadiabatic features are induced by the dynamical Franz-Keldysh effect with an anomalous band dispersion

Cavity Control of Excitons in Two-Dimensional Materials

We propose a robust and efficient way of controlling the optical spectra of two-dimensional materials and van der Waals heterostructures by quantum cavity embedding. The cavity light-matter coupling leads to the formation of exciton-polaritons, a superposition of photons and excitons. Our first-principles study demonstrates a reordering and mixing of bright and dark excitons spectral features and in the case of a type II van-der-Waals heterostructure an inversion of intra- and interlayer excitonic resonances. We further show that the cavity light-matter coupling strongly depends on the dielectric environment and can be controlled by encapsulating the active two-dimensional (2D) crystal in another dielectric material. Our theoretical calculations are based on a newly developed nonperturbative many-body framework to solve the coupled electron-photon Schrödinger equation in a quantum-electrodynamical extension of the Bethe-Salpeter approach. This approach enables the ab initio simulations of exciton-polariton states and their dispersion from weak to strong cavity light-matter coupling regimes. Our method is then extended to treat van der Waals heterostructures and encapsulated 2D materials using a simplified Mott-Wannier description of the excitons that can be applied to very large systems beyond reach for fully ab initio approaches

Floquet states in dissipative open quantum systems

We theoretically investigate basic properties of nonequilibrium steady states of periodically-driven open quantum systems based on the full solution of the Maxwell–Bloch equation. In a resonant driving condition, we find that the transverse relaxation, also known as decoherence, significantly destructs the formation of Floquet states while the longitudinal relaxation does not directly affect it. Furthermore, by evaluating the quasienergy spectrum of the nonequilibrium steady states, we demonstrate that Rabi splitting can be observed as long as the decoherence time is as short as one third of the Rabi-cycle. Moreover, we find that Floquet states can be formed even under significant dissipation when the decoherence time is substantially shorter than the cycle of driving, once the driving field strength becomes strong enough. In an off-resonant condition, we demonstrate that the Floquet states can be realized even in weak field regimes because the system is not excited and the decoherence mechanism is not activated. Once the field strength becomes strong enough, the system can be excited by multi-photon absorption and the decoherence process becomes active. As a result, the Floquet states are significantly disturbed by the environment even in the off-resonant condition. Thus, we show here that the suppression of energy transfer from light to matter is a key condition for the realization of Floquet states in both on- and off-resonant conditions not only because it prevents material damage but also because it contributes to preserving coherence

Phonoritons as Hybridized Exciton-Photon-Phonon Excitations in a Monolayer h -BN Optical Cavity

A phonoriton is an elementary excitation that is predicted to emerge from hybridization between exciton, phonon, and photon. Besides the intriguing many-particle structure, phonoritons are of interest as they could serve as functional nodes in devices that utilize electronic, phononic, and photonic elements for energy conversion and thermal transport applications. Although phonoritons are predicted to emerge in an excitonic medium under intense electromagnetic wave irradiation, the stringent condition for their existence has eluded direct observation in solids. In particular, on-resonance, intense pumping schemes have been proposed, but excessive photoexcitation of carriers prevents optical detection. Here, we theoretically predict the appearance of phonoritonic features in monolayer hexagonal boron nitride (h-BN) embedded in an optical cavity. The coherent superposition nature of phonoriton states is evidenced by the hybridization of exciton-polariton branches with phonon replicas that is tunable by the cavity-matter coupling strength. This finding simultaneously provides an experimental pathway for observing the predicted phonoritons and opens a new avenue for tuning materials properties

Unraveling materials Berry curvature and Chern numbers from real-time evolution of Bloch states

Materials can be classified by the topological character of their electronic structure and, in this perspective, global attributes immune to local deformations have been discussed in terms of Berry curvature and Chern numbers. Except for instructional simple models, linear response theories have been ubiquitously used in calculations of topological properties of real materials. Here we propose a completely different and versatile approach to obtain the topological characteristics of materials by calculating physical observables from the real-time evolving Bloch states: The cell-averaged current density reveals the anomalous velocities that lead to the conductivity quantum. Results for prototypical cases are shown, including a spin-frozen valley Hall and a quantum anomalous Hall insulator. The advantage of this method is best illustrated by the example of a quantum spin Hall insulator: The quantized spin Hall conductivity is straightforwardly obtained irrespective of the non-Abelian nature in its Berry curvature. Moreover, the method can be extended to the description of real observables in nonequilibrium states of topological materials

Time-based Chern number in periodically driven systems in the adiabatic limit

To define the topology of driven systems, recent works have proposed synthetic dimensions as a way to uncover the underlying parameter space of topological invariants. Using time as a synthetic dimension, together with a momentum dimension, gives access to a synthetic two-dimensional (2D) Chern number. It is, however, still unclear how the synthetic 2D Chern number is related to the Chern number that is defined from a parametric variable that evolves with time. Here we show that in periodically driven systems in the adiabatic limit, the synthetic 2D Chern number is a multiple of the Chern number defined from the parametric variable. The synthetic 2D Chern number can thus be engineered via how the parametric variable evolves in its own space. We justify our claims by investigating Thouless pumping in two one-dimensional (1D) tight-binding models, a three-site chain model, and a two-1D-sliding-chains model. The present findings could be extended to higher dimensions and other periodically driven configurations

Interaction and filling induced quantum phases of dual Mott insulators of bosons and fermions

Many-body effects are at the very heart of diverse phenomena found in condensed-matter physics. One striking example is the Mott insulator phase where conductivity is suppressed as a result of a strong repulsive interaction. Advances in cold atom physics have led to the realization of the Mott insulating phases of atoms in an optical lattice, mimicking the corresponding condensed matter systems. Here, we explore an exotic strongly-correlated system of Interacting Dual Mott Insulators of bosons and fermions. We reveal that an inter-species interaction between bosons and fermions drastically modifies each Mott insulator, causing effects that include melting, generation of composite particles, an anti-correlated phase, and complete phase-separation. Comparisons between the experimental results and numerical simulations indicate intrinsic adiabatic heating and cooling for the attractively and repulsively interacting dual Mott Insulators, respectively

Femtosecond exciton dynamics in WSe2 optical waveguides

Van-der Waals (vdW) atomically layered crystals can act as optical waveguides over a broad range of the electromagnetic spectrum ranging from Terahertz to visible. Unlike common Si-based waveguides, vdW semiconductors host strong excitonic resonances that may be controlled using non-thermal stimuli including electrostatic gating and photoexcitation. Here, we utilize waveguide modes to examine photo-induced changes of excitons in the prototypical vdW semiconductor, WSe2, prompted by femtosecond light pulses. Using time-resolved scanning near-field optical microscopy we visualize the electric field profiles of waveguide modes in real space and time and extract the temporal evolution of the optical constants following femtosecond photoexcitation. By monitoring the phase velocity of the waveguide modes, we detect incoherent A-exciton bleaching along with a coherent optical Stark shift in WSe2